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At least 685 records · Page 38

Performance of an i -SANEX System Based on a Water-Soluble BTP under Continuous Irradiation in a γ-Radiolysis Test Loop

Here, the i -SANEX solvent formulation consisting of nominally 0.2 M TODGA/5% 1-octanol/dodecane was γ-irradiated under realistic conditions in the Idaho National Laboratory radiolysis test loop, in contact with both extraction and stripping aqueous phases. The extraction aqueous phase was 4.5 M HNO 3 , and the stripping aqueous phase was 0.018 M SO 3 –Ph–BTP/0.35 M HNO 3 . When irradiated in contact with only the 4.5 M HNO 3 phase, the TODGA solvent maintained excellent extraction performance for americium, cerium, europium, and neodymium to a maximum absorbed dose of nearly 0.9 MGy. The results for preliminary static, batch irradiations were consistent with test loop findings. When the aqueous phase was changed to that containing the aqueous soluble BTP, the irradiated aqueous phase showed a dramatic color change, but this does not appear to have had adverse effect on solvent extraction performance. The distribution ratios for both the lanthanides and actinides were invariant with absorbed dose, and the separation factors were essentially unchanged to a maximum absorbed dose of 174 kGy. The results of inductively coupled plasma mass spectrometry analysis of the aqueous and organic phases showed that ruthenium and strontium were not extracted in the presence of the irradiated BTP-aqueous phase. Molybdenum was extracted under both conditions. Further, the buildup of corrosion products of stainless steel in the presence of the BTP was not dramatically greater than in the nitric acid-only system. Phase separation times were not adversely affected by irradiation for either system. The results presented here indicate that the performance of the TODGA/SO 3 –Ph–BTP, i -SANEX process under test loop radiolysis is much better than expected based on a literature report using single-phase batch irradiation experiments, and better than might be predicted based on diglycolamide radiolysis studies alone.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Vitrification of Hanford Tank Waste 241-AP-105 in a Continuous Laboratory-Scale Melter

Low-activity waste (LAW) stored in underground tanks on the Hanford site in Washington State is planned to be filtered for solids removal and processed through ion exchange columns for cesium removal at the Low-Activity Waste Pretreatment System facility. These pretreatment steps will allow the waste to be transferred to the Hanford Tank Waste Treatment and Immobilization Plant LAW facility for immobilization into glass. The liquid waste will be combined with glass-forming chemicals (GFCs) to form a waste feed slurry that can be fed to electric melters for vitrification. The process of continuously converting the aqueous feed slurry into a melt is dynamic and includes multiple reactions, degassing, and dissolution processes that depend on heat from the melt below. In this conversion process, waste components are partitioned into one of two streams: glass and off-gas. Processing information and chemical information associated with these waste product streams has been requested by Washington River Protection Solutions for actual tank waste from tank 241-AP-105 (referred to as AP-105). To acquire this type of information, a small-scale melter system was desired that would not require high volumes of input waste or the large resource commitment of a full-scale melter system, while also providing dynamic information that would be difficult to determine from batch reactions in a crucible system. A continuous laboratory-scale melter (CLSM), has been designed to operate with a continuous feeding process, while periodically pouring glass product and collecting off-gas. The CLSM vessel has been sized to collect the relevant process and chemical information from obtainable volumes of AP-105 waste samples. Two CLSMs were constructed: one in a non-radioactive environment for processing waste simulants and another in a fume hood capable of handling radioactive material for processing actual Hanford tank waste. This dual-system setup allowed for comparison between simulated and real tank waste with essentially identical test equipment. AP-105 waste simulant was first tested in the non-radioactive CLSM to determine the processability and desired operating window for the actual tank waste. Rhenium (Re) was added to the simulant to act as a surrogate for technetium-99 ( 99 Tc), a key waste component found in the actual tank waste. The partitioning of Re into the glass and off-gas products during the continuous feeding of simulant was determined, which allowed the Re retention, the mass flow rate of Re out of the CLSM via the glass product with respect to the mass flow rate of Re into the CLSM via the feed slurry, to be calculated. Key processing results and the average Re retention, from the CLSM test run with AP-105 simulant feed slurry are shown in Table ES.1.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A Parametric Study of Operating Carbon Anodes in the Oxide Reduction Process

A parametric study of the electrolytic reduction of uranium dioxide in molten lithium chloride – lithium oxide using carbon anodes was conducted to determine the operational parameter values necessary for high yields. Operational parameters evaluated in this study include anode and cathode current densities, anodic polarization, UO 2 batch size, and method of electrochemical control. Seven oxide reduction experiments were conducted with between 25 g and 100 g UO 2 . The current density on the cathode was the critical parameter, which indicates the reduction process is kinetically controlled by cathodic reactions. High cell currents were achieved without the application of high anodic potentials by using a large anode surface area. As a result, this approach facilitates efficient reduction at high throughput without production of chlorine or other corrosive gasses.

36 MATERIALS SCIENCE↗

Project Development of an Electrochemical Denitration and Caustic Generation System for HLW Pretreatment at Hanford - 26350

An engineering-scale electrochemical processing skid is proposed to perform the denitration of Hanford tank waste, which would help to mitigate a key process concern with the direct feed processing of the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The reduction of nitrates and organic compounds in the waste feed will directly reduce hazardous NOx and ammonia gases generated during the vitrification process, which in turn will aid in addressing potential regulatory and safety challenges associated with processing large volumes of tank waste. This paper highlights the past legacy work, project layout, accomplishments from Phase 1 and research and development envisioned for Phase 2. An innovative electrochemical denitration and caustic generation (EDCGe) process was demonstrated for the pretreatment of tank waste at the Savannah River Site (SRS) in the early 2000s. The denitration electrolyzer, off-gas abatement system, and caustic generator electrolyzer are being developed with the intent that the denitration electrolyzer will convert nitrate and nitrite anions to nitrogen gas while also yielding other gaseous byproducts, which may include N2O, NH3, VOCs, and H2. The gaseous byproducts will be managed via a tandem off-gas catalyst-bed treatment system. The caustic generation electrolyzer will recycle NaOH from the feed to produce a clean caustic stream for use within the batching tanks at Hanford, aiding in the preparation of waste for WTP. The reduction in hazardous emissions and improved waste treatment processes provides a robust solution for nuclear waste management, contributing to environmental safety and regulatory compliance. The EDCGe technology is being adapted, modified, and updated for the preparation of the Direct Feed-High Level Waste (DF-HLW) flowsheet at Hanford. Phase 1 demonstrated a bench-scale proof-of-concept for reactions involving the denitration electrolyzer and gas phase abatement of ammonia. The electrochemical technology is drawing on the scientific outcomes that were reported in the legacy work. The results from Phase 1 demonstrated the viability of the EDCGe system in reducing the nitrogen species of simple non-radioactive waste simulants. Commercially available alloys used as electrode materials and membranes are being studied for the denitration and caustic generation electrolyzers. The continuation of this project holds promise for broader applications, such as energy-efficient ammonia production, and contributes significant advancements in nuclear waste management. Additional material discovery has been investigated into ceramic Na super ion conductive (NaSICON) materials and off-gas abatement catalyst discovery. NaSICON is of interest for selective transport of Na within the electrolyzers to make a clean caustic stream. Future integration and optimization efforts, informed by Phase 1 results and ongoing research, will continue to drive advancements in nuclear waste management technology. The technology developed for the EDCGe treatment of tank waste will also have broader potential to inform other fields, such as energy-efficient ammonia production, as well as ammonia abatement catalysis through the lessons learned in electrochemical nitrate reduction. The applications and benefits of this research extend beyond Hanford and the Savannah River Site, supported by a collaborative team of scientists and engineers from national labs, academia, and industry, ensuring a comprehensive approach to solving complex waste treatment challenges. The team is leveraging advanced electrochemical technologies, machine learning, novel catalysts tailored for gaseous nitrogen species, and cutting-edge reactor systems to enhance the process efficiency and effectiveness of the denitration process.

Rodene, Dylan [Savannah River National Laboratory ↗

The Role of Retardation, Attachment and Detachment Processes during Microbial Coal-Bed Methane Production after Organic Amendment

Microbially enhanced coal-bed methane could allow for a more sustainable method of harvesting methane from un-mineable coaldbeds. The model presented here is based on a previously validated batch model; however, this model system is based on upflow reactor columns compared to previous experiments and now includes flow, transport and reactions of amendment as well as intermediate products. The model implements filtration and retardation effects, biofilm decay, and attachment and detachment processes of microbial cells due to shear stress. The model provides additional insights into processes that cannot be easily observed in experiments. This study improves the understanding of complex and strongly interacting processes involved in microbially enhanced coal-bed methane production and provides a powerful tool able to model the entire process of enhancing methane production and transport during microbial stimulation.

54 ENVIRONMENTAL SCIENCES↗

Glycolic acid physical properties and impurities assessment

This document has been revised due to recent information that the glycolic acid used in Savannah River National Laboratory (SRNL) experiments contains both formaldehyde and methoxyacetic acid. These impurities were in the glycolic acid used in the testing included in this report and in subsequent testing using DuPont (now called Chemours) supplied Technical Grade 70 wt% glycolic acid. However, these impurities were not reported in earlier revisions. Additional data concerning the properties of glycolic acid have also been added to this report. The Defense Waste Processing Facility (DWPF) is planning to implement a nitric-glycolic acid flowsheets to increase attainment to meet closure commitment dates during Sludge Batch 9. In fiscal year 2009, SRNL was requested to determine the physical properties of formic and glycolic acid blends. Blends of formic acid in glycolic acid were prepared and their physical properties tested. Increasing amounts of glycolic acid led to increases in blend density, viscosity and surface tension as compared to the 90 wt% formic acid that is currently used at DWPF. These increases are small, however, and are not expected to present any difficulties in terms of processing. The effect of sulfur impurities in Technical Grade glycolic acid was studied for its impact on DWPF glass quality. While the glycolic acid specification allows for more sulfate than the current formic acid specification, the ultimate impact is expected to be on the order of 0.033 wt% sulfur in glass. Note that lower sulfur content glycolic acid could likely be procured at some increased cost if deemed necessary. A paper study on the effects of radiation on glycolic acid was performed. The analysis indicates that substitution of glycolic acid for formic acid would not increase the radiolytic production rate of H2 and cause an adverse effect in the Slurry Receipt and Adjustment Tank (SRAT) or Slurry Mix Evaporator (SME) process. It has been cited that glycolic acid solutions that are depleted of O2 when subjected to large radiation doses produced considerable quantities of a non-diffusive polymeric material. Considering a constant air purge is maintained in the SRAT and the solution is continuously mixed, oxygen depletion seems unlikely, however, if this polymer is formed in the SRAT solution, the rheology of the solution may be affected and pumping of the solution may be hindered. However, an irradiation test with a simulated SRAT product supernate containing glycolic acid in an oxygen depleted atmosphere found no evidence of polymerization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Provenance information as a tool for addressing engineered nanoparticle reproducibility challenges

Nanoparticles of various types are of increasing research and technological importance in biological and other applications. Difficulties in the production and delivery of nanoparticles with consistent and well defined properties appear in many forms and have a variety of causes. Among several issues are those associated with incomplete information about the history of particles involved in research studies including the synthesis method, sample history after synthesis including time and nature of storage and the detailed nature of any sample processing or modification. In addition, the tendency of particles to change with time or environmental condition suggests that the time between analysis and application is important and some type of consistency or verification process can be important. The essential history of a set of particles can be identified as provenance information tells the origin or source of a batch of nano-objects along with information related to handling and any changes that may have taken place since it was originated. A record of sample provenance information for a set of particles can play a useful role in identifying some of the sources and decreasing the extent of particle variability and the observed lack of reproducibility observed by many researchers.

Environmental Molecular Sciences Laboratory↗

Investigation of the Effect of Chrome and Nickel Concentrations During Two-Piston Splat Quenching of Austenitic Stainless Steels

For solidification rates at or near equilibrium solidification conditions the effects of chrome (Cr) and nickel (Ni) on stainless steel solidification modes and microstructures are well detailed. However, fusion-based additive manufacturing (FBAM) processes that rely on faster, more rapid solidification rates call for a more in-depth understanding of the effects of rapid solidification on the solidification behavior and how these change with variations in alloy composition. Eleven custom stainless steel (SS) alloys with unique compositions based on 316L were made using targeted alloying element additions to generate feedstock with Cr/Ni eq ratios ranging from 0.9 to 2.1. Two-piston splat quenching (SQ) was used to produce rapid solidification conditions similar to those achieved in powder bed fusion processes in a fraction of the time and cost of traditional methods. Employing heat transfer simulations, SEM, TEM, and STEM characterization techniques, the SQ process was found to consistently produce solidification rates estimated to be between ~ 0.4 and 1.6 m/s. Five unique solidification microstructures were identified within the rapidly solidified SQ samples (primary austenite, massively transformed ferrite to austenite, primary austenite and massively transformed ferrite to austenite, primary ferrite, and primary ferrite and massively transformed ferrite to austenite). Both the primary ferrite solidification mode and primary ferrite phase were found to form at lower Cr/Ni eq values than previously predicted. SQ samples with compositions that were within the compositional specifications for 316L SS, an alloy which is commonly used in FBAM processes, demonstrated a wider range of potential solidification modes and microstructures that could form at rapid solidification rates than expected. Finally, by using SQ as a means to simulate rapid solidification conditions similar to those observed in FBAM processes, potential new alloy compositions can be screened faster and more cost effectively than purchasing and running test batches of the metallic powder.

36 MATERIALS SCIENCE↗

Implementation of McMurchie–Davidson Algorithm for Gaussian AO Integrals Suited for SIMD Processors

We report an implementation of the McMurchie− Davidson evaluation scheme for 1- and 2-particle Gaussian AO integrals designed for processors with Single Instruction Multiple Data (SIMD) instruction sets. Like in our recent MD implementation for graphical processing units (GPUs) [Asadchev, A.; Valeev, E. F.. J. Chem. Phys. 2024, 160, 244109.], variable-sized batches of shellsets of integrals are evaluated at a time. By optimizing for the floating point instruction throughput rather than minimizing the number of operations, this approach achieves up to 50% of the theoretical hardware peak FP64 performance for many common SIMD-equipped platforms (AVX2, AVX512, NEON), which translates to speedups of up to 30 over the state-of-the-art one-shellset-at-a-time implementation of Obara−Saika-type schemes in Libint for a variety of primitive and contracted integrals. As with our previous work, we rely on the standard C++ programming language such as the std::simd standard library feature to be included in the 2026 ISO C++ standard without any explicit code generation to keep the code base small and portable. The implementation is part of the open source LibintX library freely available at https://github.com/ValeevGroup/libintx.

Basis sets↗

Silver-Loaded Xerogel Nanostructures for Iodine Capture: A Comparison of Thiolated versus Unthiolated Sorbents

Here this paper describes the development and provides comparisons of thiolated (-SH) and unthiolated Ag-Al-Si-O xerogels for iodine gas capture. These xerogels were produced from alkoxides and then heat-treated at 350 °C to provide mechanical strength for subsequent processing steps. Then, a portion of the xerogels was thiolated using (3-mercaptopropyl)trimethoxysilane. Next, thiolated and unthiolated batches were ion-exchanged in AgNO 3 solutions where Ag + replaced Na + in the gel network on a near 1:1 molar basis. Subsamples of the Ag-exchanged xerogels were subjected to a reduction step in H 2 /Ar to convert Ag + to Ag 0 where the rest of the Ag-exchanged (Ag + ) were not reduced. X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy revealed nanoscale Ag 0 in the Ag + samples despite no active reduction where actively reduced samples had bimodal Ag 0 distribution of ~2-3 nm hexagonal and ~6-7 nm cubic crystallites. Synchrotron X-ray absorption spectroscopy was used to assess the oxidization states of Ag, S, and I within the different xerogel samples. The specific surface areas of the base xerogels decreased as subsequent treatments were performed on the as-made samples, albeit the decreases were smaller than aerogel equivalents of these samples from a previous study. All iodine-loaded Ag-based samples showed a mixture of β-AgI and γ-AgI. Comparisons of iodine-loading results with other Ag-based iodine sorbents show that the thiolated Ag 0 -xerogels in this work have one of the highest iodine-loading capacities (q e ) reported to date in saturated conditions with the thiolated Ag 0 -xerogel showing 522 mg iodine per g of the sorbent.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Adsorption of Cu(II) on Oxidized Multi-Walled Carbon Nanotubes in the Presence of Hydroxylated and Carboxylated Fullerenes

The adsorption of Cu(II) on oxidized multi-walled carbon nanotubes (oMWCNTs) as a function of contact time, pH, ionic strength, temperature, and hydroxylated fullerene (C 60 (OH) n ) and carboxylated fullerene (C 60 (C(COOH) 2 ) n ) were studied under ambient conditions using batch techniques. The results showed that the adsorption of Cu(II) had rapidly reached equilibrium and the kinetic process was well described by a pseudo-second-order rate model. Cu(II) adsorption on oMWCNTs was dependent on pH but independent of ionic strength. Compared with the Freundlich model, the Langmuir model was more suitable for analyzing the adsorption isotherms. The thermodynamic parameters calculated from temperature-dependent adsorption isotherms suggested that Cu(II) adsorption on oMWCNTs was spontaneous and endothermic. The effect of C 60 (OH) n on Cu(II) adsorption of oMWCNTs was not significant at low C 60 (OH) n concentration, whereas a negative effect was observed at higher concentration. The adsorption of Cu(II) on oMWCNTs was enhanced with increasing pH values at pH < 5, but decreased at pH ≥ 5. The presence of C 60 (C(COOH) 2 ) n inhibited the adsorption of Cu(II) onto oMWCNTs at pH 4–6. The double sorption site model was applied to simulate the adsorption isotherms of Cu(II) in the presence of C 60 (OH) n and fitted the experimental data well.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Recommendations for Reduction in Radionuclide Analyte Analysis in Support of WTP Operations

In support of Hanford Tank Waste Treatment and Immobilization Plant (WTP) direct feed low-activity waste operations, this document seeks to provide a discussion on currently required radionuclide sample analyses and which, if any, are planned but may not be needed. The total number of analyses is more than 10,000 per year and, often, this analytical endeavor is difficult due to troublesome components. Such components cause issues due to low concentrations, difficulty of analysis, lack of standards, or other reasons. One of the main goals is to remove onerous or troublesome components that are present in low enough concentrations to not pose a threat of the resulting waste form being non-compliant if not measured. Additionally, if it can be demonstrated that the large number of analyses is not needed, then that will save hold times in operations, decrease the amount of money required for operations, and reduce potential exposure for plant staff or researchers. Suggestions are provided for radionuclide analytes that may not be needed and can be safely estimated from process knowledge documented in the best basis inventory. The analytes recommended for removal were determined via calculations using batch feed estimates from the Tank Utilization Assessment of 2013. Approximately 750 feed estimates, representing waste compositions throughout the lifetime of the Hanford mission, were analyzed, and radionuclide concentrations were compared against established reporting and contractual limits as specified in the WTP contract. Analytes that were found to be consistently below the limits include many transuranic radionuclides and other radionuclides present in the waste in small concentrations. A total of 23 of the 44 radionuclides in the batch estimates were not significant in all batch feeds.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

OLCF’s Advanced Computing Ecosystem (ACE): FY25 Update for Ongoing Efforts

The advent of widespread use of artificial intelligence (AI) and machine learning (ML) models in science, coupled with fast data production rates of scientific instruments strain the traditional batch-oriented high-performance computing (HPC) environment. As scientific exploration continues to require more data and faster processing and analysis, new emerging technologies and capabilities to enable cross-facility and time-sensitive workflows are required for seamless integration of HPC and experimental facilities. The Advanced Computing Ecosystem (ACE) is a strategic initiative within the Oak Ridge Leadership Computing Facility (OLCF) established in 2024 to support the development of cutting-edge technologies to advance computational research and infrastructure at OLCF and across the Department of Energy (DOE). Several DOE initiatives are spearheading the evolution of the scientific landscape by blurring facility boundaries and connecting the user facilities to advance scientific capabilities and ensure energy dominance. The DOE Integrated Research Infrastructure (IRI) program is one example that is laying a foundation to support complex cross-facility workflows. The IRI program aims to integrate diverse computational resources, data infrastructures, and scientific instruments to facilitate collaboration and accelerate scientific discovery. The Interconnected Science Ecosystem (INTERSECT) initiative at Oak Ridge National Laboratory (ORNL) is another example that aims to revolutionize scientific research through AI-driven, interconnected autonomous laboratories and research facilities. Finally, the American Science Cloud (AmSC), recently announced in the “One Big Beautiful Bill”, aims to leverage prior infrastructure efforts of the IRI and automation and AI efforts of INTERSECT (and others) to build a federated, AI-augmented AmSC platform to unify the DOE’s computing, experimental, and data resources to catalyze scientific innovation.

97 MATHEMATICS AND COMPUTING↗

Development and Implementation of an Automatic Continuous Online Monitoring and Control Platform for Polymerization Reactions to Sharply Boost Energy and Resource Efficiency in Polymer Manufacturing

The project goal was to create an energy saving paradigm shift in how polymers are manufactured in the 21st century. It used Automatic Continuous Online Monitoring of Polymerization reactions (ACOMP) integrated for the first time with automatic active control to create the innovative ‘ACOMP/Control Interface’, or ‘ACOMP/CI’. ACOMP/CI will begin the transformation from old, inefficient processes into highly evolved, energy and resource efficient ones. The ACOMP platform is broadly applicable to many types of reactions and processes throughout the vast polymer industry. The industry provides materials for sectors such as automotive, aerospace, oil recovery, agriculture, paints, resins, adhesives, pharmaceuticals and therapeutic proteins, optics, electronics, lightweight building materials, and many more. The U.S. chemical industry is one of the last major sectors in which the U.S. has top global stature. It consumes 24% of all U.S. manufacturing energy, produces over $800B of product annually, supports 25% of the U.S. GDP and employs over 6 million people. It is also a major source of GHG emissions. Polymers make up approximately 30% of this sector. It is estimated that annually 60 TBtu of energy could be saved and 3 million tons less of GHG emissions produced by optimizing production in the polyolefin manufacturing sector alone. The project scope included first time design and prototyping of an ACOMP/CI, creation of active reaction controllers, and demonstration of control capabilities on ideal, low concentration polymerization reactions. All these elements of the scope were met, including advances and findings not originally anticipated. Extensions to more complex reactions, beyond the reactor capabilities of the current project ACOMP/CI, such as polyolefins and other high pressure/high temperature reactions, are being proposed in Fall 2017 to CESMII, a DoE based NNMI. The initial proposal was for a three year funded project, but this was reduced to a two year project and budget due to funding constraints. Hence, some of the original plans, such as adaptation of the ACOMP/CI to more relevant industrial processes, such as emulsion and dispersion technologies, could not be carried out. A third year of funding was requested at the end of the project, but DoE did not have resources to grant this. The sub-contractor Fluence Analytics (previously Advanced Polymer Monitoring Technologies, Inc) designed, prototyped, and commissioned a working ACOMP/CI by June 2015. The reaction characteristics to be automatically controlled were i) conversion kinetics, ii) molecular weight, iii) copolymer composition, and iv) simultaneous molecular weight and composition. A two pronged control strategy was used. The Tulane/Fluence group took a basic principles approach that did not rely on kinetic models. The LSU group took a more complex, non-linear model-oriented approach involving complete kinetic descriptions of the reaction system Each of these approaches proved successful in their own way. By April 2016 fully automatic control of conversion and weight average molecular weight, Mw, trajectories was achieved using the Tulane/Fluence (TF) basic principles controller. Similar results were obtained by the LSU non-linear model controller by August 2016. The demonstration system was aqueous free radical polymerization of acrylamide, Am. The control variables were temperature and semi-batch feed to the reactor of Am monomer and initiator. A demonstration of active manual conversion control in an industrial process using high solids in inverse emulsion polymerization of Am was achieved. During Summer 2016 the TF controller was used in conjunction with a chain transfer agent, another control variable, to automatically produce multi-modal molecular weight distributions, MWD, in a single reactor. Industrially, multi-modal MWD are produced by mixing products made in separate reactors, requiring significant extra time, energy, and reactor resources. Recognizing the industrial potential a patent on automatic production of multi-modal polymers was filed, and DoE acknowledged. In Fall 2016 the TF team developed a basic principles controller for copolymer composition and demonstrated it on aqueous free radical copolymerization of comonomers Am and styrene sulfonate, SS. TF then fused the Mw and composition controllers to achieve simultaneous control of both Mw and copolymer composition trajectories. Numerous simultaneous trajectories were demonstrated, including a trimodal composition distribution with constant Mw. Meanwhile, the LSU group developed a Kalman filter to improve the results of their automatic Mw and conversion controller and successful tests were made. During the project the TF team developed a means of computing full MWD during polymer synthesis without need for any chromatographic separation, based on model distributions. This means the polymer product is ‘born characterized’ and this can eliminate post-manufacture analytical laboratory quality control. TF filed a joint patent application on this new approach to chromatography-free determination of MWD with acknowledgment to DoE. The Tulane group obtained a 60MHz NMR during the project and recently completed the first work on separating three comonomers, Am, SS, and Na-acrylate, with a first demonstration of terpolymer composition control with the TF basic principles controller. Widespread dissemination of ACOMP/CI in the polymer manufacturing sector will bolster DoE goals of energy efficiency and reduced GHG emissions: The ability to monitor and actively control polymerization reactions will lead to more efficient use of energy and non-renewable resources, plant and labor time, increase the safety of manufacturing personnel, and will enhance product quality and lead to feasibility of manufacturing of polymers currently too complex for industrial scale production, while leading to less GHG emissions per kilo of product, and allowing for increased U.S. competitiveness in this enormous manufacturing sector. When ACOMP/CI is expanded to the polyolefin industry it is estimated that 60 TeraBTU/year of energy can be saved. Much of this saving is anticipated to come from optimized control of grade changeovers in steady state reactors and maintenance of steady states. Conclusions: ACOMP’s ability to provide continuous realtime data streams of measured polymer and reaction characteristics made it possible, for the first time, to directly and automatically control free radical polymerization reactions. An industrial client of Fluence Analytics has requisitioned the first ACOMP/CI which uses the TF basic principles controller. This sets the stage for FA to add control features to the ACOMP systems it has begun to install on the industrial scale beginning in 2014. Recommendations: This successful project was mainly limited to ideal polymerizations not of an industrial sort. The most energy intensive portion of polymer manufacturing is polyolefins. Adoption of ACOMP/CI to this enormous industrial sector faces the enormous challenges of high temperature, high pressure continuous sampling and high temperature sensor operation to obtain the continuous data needed for direct reaction control. The project team has a strategy for achieving this ambitious goal and will present it in Fall 2017 as a proposal to CESMII/DoE. It is recommended that this upcoming proposal be funded in order to make full use of the achievements of this just ended DoE project as the next step towards making polyolefin ACOMP/CI an energy saving reality. It is projected that ACOMP/CI can have its first polyolefin testbed demonstrations within two years of beginning the proposed project.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Adsorption of La(III) in aqueous systems by N-(2-hydroxyethyl) salicylaldimine-functionalized mesoporous silica

Highlights: • HESI-SBA-15 as a new adsorbent was synthesized for the first time. • This adsorbent was selective for lanthanum ion removal in presence of other ions. • The factors that affected adsorption of La(III) in aqueous solution were studied. • La{sup 3+} uptake process was according to pseudo-second-order kinetic model. - Abstract: In this work, a novel modified SBA-15 with covalently bonded N-(2-hydroxyethyl) salicylaldimine Schiff base as a ligand (HESI-SBA-15) was successfully synthesized, characterized and used as a selective absorbent for lanthanum ions removal from water systems. The structure and physicochemical properties were identified by elemental analysis, X-ray diffraction, nitrogen adsorption–desorption, thermogravimetric analysis and FTIR spectroscopy, scanning electron microscopy, BET surface area and BJH pore size. These techniques have confirmed that the Schiff base ligand was successfully grafted on the SBA-15 surface and ordered arrangement of the silica support was preserved under functionalization. The effect of pH, adsorbent dose, contact time, ionic strength and initial metal ions concentration were studied by using a batch method. This new adsorbent showed high adsorption capacity and selectivity for lanthanum in the presence of other ions. The adsorption process was exactly according to the pseudo-second-order kinetic model. The adsorbent showed a good reusability after four cycles recovery.

36 MATERIALS SCIENCE↗

Lipids from High-Protein Algae Biomass

Biofuels from renewable and sustainable sources will be a critical component of reducing greenhouse gasses. To this end, in achieving maximum biomass productivity in outdoor ponds at a reasonable cost, algae must be grown at a maximal rate. This current algae cultivation strategy results in high-protein biomass because there is insufficient time for deplete-hold steps that increase lipids but also cost. Thus methods to convert high-protein (>50%) need to be developed for biofuels. The Consolidated Algae Processing (CAP) strategy has previously shown utility on high-carbohydrate algae biomass and has now been expanded to include methods aimed at converting the protein fraction to lipids. After acid-pretreatment, hydrolysate liquor is oxidatively treated to deaminate and convert soluble proteins and amino acids into four main carboxylate acids; formic, acetic, succinic, and propionic. These acids are readily and completely fermented into intracellular lipids using oleaginous yeast. Using a fed-batch fermentation strategy and no added nutrients, we achieved nearly 30% intracellular lipids and 1.3 g/L lipids demonstrating the potential of our expanded CAP process to generate additional lipids for conversion to biofuels as part of an algae-focused biorefinery.

AAD↗

Characterization of DWPF recycle condensate tank materials

A Defense Waste Processing Facility (DWPF) Recycle Condensate Tank (RCT) sample was delivered to the Savannah River National Laboratory (SRNL) for characterization with particular interest in the concentration of I-129, U-233, U-235, total U, and total Pu. Since a portion of Salt Batch 8 will contain DWPF recycle materials, the concentration of I-129 is important to undertand for salt batch planning purposes. The chemical and physical characterizations are also needed as input to the interpretation of future work aimed at determining the propensity of the RCT material to foam, and methods to remediate any foaming potential. According to DWPF the Tank Farm 2H evaporator has experienced foaming while processing DWPF recycle materials. The characterization work on the RCT samples has been completed and is reported here. The composition of the Sludge Batch 8 (SB8) RCT material is largely a low base solution of 0.2M NaNO 2 and 0.1M NaNO 3 with a small amount of formate present. Insoluble solids comprise only 0.05 wt.% of the slurry. The solids appear to be largely sludge-like solids based on elemental composition and SEM-EDS analysis. The sample contains an elevated concentration of I-129 (38x) and substantial 59% fraction of Tc-99, as compared to the incoming SB8 Tank 40 feed material. The Hg concentration is 5x, when compared to Fe, of that expected based on sludge carryover. The total U and Pu concentrations are reduced significantly, 0.536 wt.% TS and 2.42E-03 wt.% TS, respectively, with the fissile components, U-233, U-235, Pu-239, and Pu-241, an order of magnitude lower in concentration than those in the SB8 Tank 40 DWPF feed material. This report will be revised to include the foaming study requested in the TTR and outlined in the TTQAP when that work is concluded.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Full-Scale Testing of the Ambient Pressure, Acid-Dissolution Front-End Process for the Current 99 Mo Recovery Processes

The Global Threat Reduction Initiative (GTRI) Conversion Program is actively developing technologies for converting civilian facilities that use high enriched uranium (HEU) to low enriched uranium (LEU) fuels and targets. The conversion of conventional HEU targets to LEU for the production of 99 Mo production requires approximately five times the uranium in a target to maintain the 99 Mo yield on a per-target basis. Under GTRI, Argonne National Laboratory (Argonne) is developing two frontend options for current 99 Mo production processes to allow the use of LEU-foil targets. In both processes, the aim is to produce a frontend product that is compatible with current 99 Mo purification operations and will provide the same or a higher yield of 99 Mo for the same number of irradiated targets. The two frontend processes under development as part of this project are (1) the dissolution of irradiated LEU foil (up to 250 g in a single batch) and nickel fission recoil barrier in nitric acid at ambient pressure; and (2) the electrochemical dissolution of LEU foil in series of steps that produces an alkaline (basic) solution feed for 99 Mo purification. This report describes results from performance tests and design optimization of the ambient pressure, nitric-acid-dissolver system. The design, fabrication, and performance test planning for this system are described in more detail in previous reports (Jerden et al. 2011a,b, 2012). Full-scale demonstrations of both of the frontend processes using irradiated uranium foils are planned to be performed at Oak Ridge National Laboratory this fiscal year.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗